Affiliation:
1. Department of Chemistry MOE Key Laboratory of Organic OptoElectronics and Molecular Engineering Tsinghua University 100084 Beijing China
2. Division of Chemistry and Chemical Engineering California Institute of Technology Pasadena California 91125 USA
3. Department of Chemistry and Biochemistry University of Oklahoma Norman Oklahoma 73019 USA
4. SINOPEC Research Institute of Petroleum Processing Co., Ltd Beijing 100083 China
5. School of Science and Engineering The Chinese University of Hong Kong Shenzhen 518172 Guangdong China
Abstract
AbstractIn microcavity, strong coupling between light and molecules leads to the formation of hybrid excitations, i. e., the polaritons, or exciton‐polaritons. Such coupling may alter the energy landscape of the system and the optical properties of the material, making it an effective approach for controlling the light emission from molecular materials. However, due to the complexity of vibrational modes, spectroscopic calculations for organic exciton‐polaritons remain to be challenging. In this work, based on the linear‐response quantum‐electrodynamical time‐dependent density functional theory (QED‐TDDFT), we employ the thermal vibrational correlation function (TVCF) formalism to calculate the molecular optical spectrum of the lower polaritons (LP) at first‐principles level for three molecules, i. e., anthracene, distyrylbenzenes (DSB), and rubrene. The polaron decoupling effect is confirmed from our first‐principles computations. The theoretical emission spectra of LP provide new insights for aiding molecular and device design in microcavities that are otherwise hindered due to the lack of vibrational information.
Funder
National Science Foundation